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US4409041A - Amorphous alloys for electromagnetic devices - Google Patents

Amorphous alloys for electromagnetic devices Download PDF

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Publication number
US4409041A
US4409041A US06/286,918 US28691881A US4409041A US 4409041 A US4409041 A US 4409041A US 28691881 A US28691881 A US 28691881A US 4409041 A US4409041 A US 4409041A
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alloy
recited
alloys
discrete particles
average
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Expired - Lifetime
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US06/286,918
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Inventor
Amitava Datta
Lance A. Davis
Nicholas J. DeCristofaro
Jordi Marti
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Honeywell International Inc
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Allied Corp
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Assigned to ALLIED CORPORATION reassignment ALLIED CORPORATION ASSIGNMENT OF ASSIGNORS INTEREST. Assignors: DATTA, AMITAVA, DAVIS, LANCE A., DE CRISTOFARO, NICHOLAS J., MARTI, JORDI
Priority to US06/286,918 priority Critical patent/US4409041A/en
Priority to AT81107315T priority patent/ATE21417T1/de
Priority to DE8181107315T priority patent/DE3175108D1/de
Priority to EP81107315A priority patent/EP0049770B1/en
Priority to AU75554/81A priority patent/AU551753B2/en
Priority to KR1019810003573A priority patent/KR890001340B1/ko
Priority to CA000386675A priority patent/CA1181262A/en
Priority to ES505808A priority patent/ES8206642A1/es
Publication of US4409041A publication Critical patent/US4409041A/en
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/18—Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/32—Ferrous alloys, e.g. steel alloys containing chromium with boron
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C45/00—Amorphous alloys
    • C22C45/02—Amorphous alloys with iron as the major constituent
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/147—Alloys characterised by their composition
    • H01F1/153—Amorphous metallic alloys, e.g. glassy metals
    • H01F1/15341—Preparation processes therefor

Definitions

  • the invention relates to iron-boron base amorphous metal alloy compositions and, in particular, to amorphous alloys containing iron, boron, silicon and carbon having enhanced high frequency magnetic properties.
  • An amorphous material substantially lacks any long range atomic order and is characterized by an X-ray diffraction profile consisting of broad intensity maxima. Such a profile is qualitatively similar to the diffraction profile of a liquid or ordinary window glass. This is in contrast to a crystalline material which produces a diffraction profile consisting of sharp, narrow intensity maxima.
  • amorphous materials exist in a metastable state. Upon heating to a sufficiently high temperature, they crystallize with evolution of the heat of crystallization, and the X-ray diffraction profile changes from one having amorphous characteristics to one having crystalline characteristics.
  • Novel amorphous metal alloys have been disclosed by H.S. Chen and D.E. Polk in U.S. Pat. No. 3,856,513, issued Dec. 24, 1974. These amorphous alloys have the formula M a Y b Z c where M is at least one metal selected from the group of iron, nickel, cobalt, chromium and vanadium, Y is at least one element selected from the group consisting of phosphorus, boron and carbon, Z is at least one element selected from the group consisting of aluminum, antimony, beryllium, germanium, indium, tin and silicon, "a” ranges from about 60 to 90 atom percent, "b” ranges from about 10 to 30 atom percent and "c” ranges from about 0.1 to 15 atom percent.
  • amorphous alloys have been found suitable for a wide variety of applications in the form of ribbon, sheet, wire, powder, etc.
  • the Chen and Polk patent also discloses amorphous alloys having the formula T i X j , where T is at least one transition metal, X is at least one element selected from the group consisting of aluminum, antimony, beryllium, boron, germanium, carbon, indium, phosphorus, silicon and tin, "i” ranges from about 70 to 87 atom percent and "j" ranges from about 13 to 30 atom percent.
  • T is at least one transition metal
  • X is at least one element selected from the group consisting of aluminum, antimony, beryllium, boron, germanium, carbon, indium, phosphorus, silicon and tin
  • "i” ranges from about 70 to 87 atom percent
  • "j" ranges from about 13 to 30 atom percent.
  • an iron based boron containing magnetic alloy having at least 85 percent of its structure in the form of an amorphous metal matrix, the alloy is annealed at a temperature and for a time sufficient to induce precipitation of discrete particles of its induce precipitation of discrete particles of its constituents.
  • Precipitated discrete particles of the alloy have an average size ranging from about 0.05 ⁇ m to 1 ⁇ m and an average interparticle spacing of about 1 ⁇ m to about 10 ⁇ m, and constitute an average volume fraction of the alloy of about 0.01 to 0.3.
  • Annealing of the alloy is conducted in the presence of a magnetic field.
  • the alloy is composed of a composition having the formula Fe a B b Si c C d wherein "a”, “b”, “c”, and “d” are atomic percentages ranging from about 74 to 84, 8 to 24, 0 to 16 and 0 to 3, respectively, with the proviso that the sum of "a", "b", “c” and “d” equals 100.
  • the invention provides a method of enhancing magnetic properties of the alloy set forth above, which method comprises the steps of (a) quenching a melt of the alloy at a rate of about 10 5 ° to 10 6 ° C./sec to form said alloy into continuous ribbon; (b) coating said ribbon with an insulating layer such as magnesium oxide; (c) annealing said coated ribbon at a temperature and for a time sufficient to induce precipitation of discrete particles in the amorphous metal matrix thereof.
  • Alloys produced in accordance with the method of this invention are not more than 30 percent crystalline and preferably not more than about 15 percent crystalline as determined by X-ray diffraction, electron diffraction, or transmission electron microscopy.
  • Alloys produced by the method of this invention exhibit improved high frequency magnetic properties that remains stable at temperatures up to about 150° C.
  • the alloys are particularly suited for use in energy storage inductors, pulse transformers, transformers for switch mode power supplies, current transformers and the like.
  • FIG. 1 is a graph showing the relationship between induction and magnetizing force for amorphous alloys in which precipitated discrete crystalline particles are absent;
  • FIG. 2 is a graph showing the relationship between induction and magnetizing force for amorphous alloys of the present invention containing an optimum volume fraction of discrete particles;
  • FIG. 3 is a graph showing the relationship between induction and magnetizing force for amorphous alloys of the invention containing a volume fraction of discrete particles larger than the optimum amount;
  • FIG. 4 is a schematic representation of an alloy of the invention, showing the distribution of discrete particles therein.
  • composition of the new iron based amorphous alloys preferably consists essentially of 74 to 84 atom percent iron, 8 to 24 atom percent boron, 0 to 16 atom percent silicon and 0 to 3 atom percent carbon.
  • Such compositions exhibit enhanced high frequency magnetic properties when annealed in accordance with the method of the invention. The improved magnetic properties are evidenced by high magnetization, low core loss and low volt-ampere demand.
  • An especially preferred composition within the foregoing ranges consists of 79 atom percent iron, 16 atom percent boron, 5 atom percent silicon and 0 atom percent carbon.
  • Alloys treated by the method of the present invention are not more than 30 percent crystalline and preferably are about 15 percent crystalline. High frequency magnetic properties are improved in alloys possessing the preferred volume percent of crystalline material.
  • the volume percent of crystalline material is conveniently determined by X-ray diffraction, electron diffraction or transmission electron microscopy.
  • the amorphous metal alloys are formed by cooling a melt at a rate of about 10 5 ° to 10 6 ° C./sec.
  • the purity of all materials is that found in normal commercial practice.
  • a variety of techniques are available for fabricating splat-quenched foils and rapid-quenched continuous ribbons, wire, sheet, etc.
  • a particular composition is selected, powders or granules of the requisite elements (or of materials that decompose to form the elements, such as ferroboron, ferrosilicon, etc.) in the desired proportions are melted and homogenized, and the molten alloy is rapidly quenched on a chill surface, such as a rotating cylinder.
  • the magnetic properties of the subject alloys can be enhanced by annealing the alloys.
  • the method of annealing generally comprises heating the alloy to a temperature for a time to induce precipation of discrete crystalline particles within the amorphous metal matrix, such particles having an average size ranging from about 0.05 to 1 ⁇ m, an average interparticle spacing of about 1 to 10 ⁇ m and constituting an average volume fraction of about 0.01 to 0.3%.
  • the annealing step is typically conducted in the presence of a magnetic field, the strength of which ranges from about 1 Oersted (80 amperes per meter) to 10 Oersteds (800 amperes per meter).
  • excellent magnetic properties are obtained and manufacturing costs are reduced by annealing the alloy in the absence of a magnetic field.
  • the d.c. B-H loop is sheared with substantially reduced B r , as in FIG. 2.
  • sheared d.c. B-H loops will be referred to as Type B.
  • Sheared loop material exhibits increased low field permeabilities and reduced core losses at high frequencies.
  • the high frequency core loss of sheared loop material is approximately one-half the loss of square loop material.
  • Lower core loss results in less heat build-up in the core and permits the use of less core material at a higher induction level for a given operating temperature.
  • the d.c. B-H loop becomes flat with near zero B r , as shown in FIG. 3.
  • flat d.b. B-H loops will be referred to as Type C.
  • the exciting power necessary to drive flat loop material is extremely large, reaching values up to ten times the exciting power of sheared or square loop material.
  • the dominant component of the total core loss is the eddy current loss, which decreases with the ferromagnetic domain size.
  • the domain size can be reduced by controlled precipitation of discrete ⁇ -(Fe, Si) particles, which act as pinning points for the domain walls.
  • the extent to which core loss is minimized by controlled precipitation in accordance with the invention depends upon the interparticle spacing, volume fraction of the discrete particles and particle size of the precipitated phase. Because the particles act as the pinning points for the domain walls, the domain size is controlled by the interparticle spacing. Generally, the interparticle spacing should be of the same order of the domain size. Absent the presence of discrete particles, the domain size is too large, with the result that eddy current and core losses are excessive. However, too small an interparticle spacing results in very small domains and impedes the domain wall motion, raising the high frequency core loss. Preferably the interparticle spacing should range from about 2 to 6 ⁇ m.
  • the extent to which core loss is minimized depends upon the alloy's volume fraction of discrete ⁇ -(Fe, Si) particles. When the volume fraction increases beyond 30%, the soft magnetic characteristics of the amorphous matrix begin to deteriorate and the crystalline ⁇ -(Fe, Si) particles offer excessive resistance to the domain wall motion. It has been found necessary to control the volume fraction of the discrete crystalline particles within a range of about 1-30%.
  • the volume fraction is a function of the interparticle spacing and particle size. It has been found that the particle size preferably ranges from about 0.1 to 0.5 ⁇ m.
  • torodial samples For amorphous alloys containing about 78 to 82 atom percent iron, 10 to 16 atom percent boron, 3 to 10 atom percent silicon and 0 to 2 atom percent carbon, torodial samples must be heated to temperatures between about 340° C. and 450° C. for times from about 15 minutes to 5 hours to induce the optimum distribution of discrete crystalline particles. The specific time and temperature is dependent on alloy composition and quench rate.
  • the discrete crystalline particles are star shaped, ⁇ - (Fe, Si) precipitates, as illustrated in FIG. 4. The precipitate size ranges from about 0.1 to 0.3 ⁇ m.
  • the preferred average interparticle spacing (d) ranges from about 1.0 to 10. ⁇ m, corresponding to an optimum volume fraction of about 0.01 to 0.15. To calculate interparticle spacing from election micrographs, care must be taken to account for the projection of three dimensional arrays onto a two dimensional image.
  • alloys annealed by the method of the present invention exhibit improved magnetic properties that are stable at temperatures up to about 150° C.
  • the temperature stability of the present alloys allows utilization thereof in high temperature applications.
  • cores comprising the subject alloys When cores comprising the subject alloys are utilized in electromagnetic devices, such as transformers, they evidence low power loss and low exciting power demand, thus resulting in more efficient operation of the electromagnetic device.
  • Cores made from the subject alloys require less electrical energy for operation and produce less heat.
  • cooling apparatus is required to cool the transformer cores, such as transformers in aircraft and large power transformers, an additional savings is realized since less cooling apparatus is required to remove the smaller amount of heat generated by cores made from the subject alloys.
  • the high magnetization and high efficiency of cores made from the subject alloys result in cores of reduced weight for a given capacity rating.
  • Toroidal test samples were prepared by winding approximately 0.030 kg of 0.0254 m wide alloy ribbon of the composition Fe 81 B 13 .5 Si 3 .5 C 2 on a steatite core having inside and outside diameters of 0.0397 m and 0.0445 m, respectively.
  • the alloy was cast into ribbon by quenching the alloy on a chromium coated copper substrate.
  • One hundred and fifty turns of high temperature magnetic wire were wound on the toroid to provide a d.c. circumferential field of up to 795.8 ampere/meter for annealing purposes.
  • the samples were annealed in an inert gas atmosphere at temperatures from 365° C. to 430° C. for times from 30 minutes to 2 hours with the 795.8 A/m field applied during heating and cooling.
  • the average particle size, interparticle distance and volume fraction were measured by transmission electron microscopy. These parameters plus the 50 kHz, 0.11 power loss and exciting power are set forth in Table I as a function of the annealing parameters
  • Toroidal test samples were prepared in accordance with the procedure set forth in Example I, except that the alloy was cast into ribbon by quenching the alloy on a Cu-Be substrate of higher conductivity than the substrate of Example I.
  • the average particle size inter-particle distance, volume fraction, power loss and exciting power of the alloys are set forth in Table II.
  • Toroidal test samples (hereafter designated Examples 3-4 were prepared in accordance with the same procedure set forth in Example II except that the composition of the alloy quenched into ribbon was Fe 81 B 14 Si 5 and Fe 78 B 16 Si 5 , respectively.
  • Power loss and exciting power values for these alloys at 50 kHz and 0.1 T are set forth in Tables III and IV as a function of annealing temperatures.
  • Toroidal test samples of alloy Fe 79 B 16 Si 5 were prepared in accordance with the procedure set forth in Example I, except that the alloy was cast into ribbon by quenching the alloy on a Cu-Be substrate of higher conductivity than the substrate of Example I. Also, unlike Examples I and II, test samples were annealed in the absence of a magnetic field. Microstructural characteristics namely, the average particle size, inter-particle distance and volume fraction remained substantially the same as shown in Table IV. Power loss and exciting power values for the alloy at 50 KHz and 0.1 T are set forth in Table V as a function of annealing conditions.

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  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
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US06/286,918 1980-09-26 1981-07-29 Amorphous alloys for electromagnetic devices Expired - Lifetime US4409041A (en)

Priority Applications (8)

Application Number Priority Date Filing Date Title
US06/286,918 US4409041A (en) 1980-09-26 1981-07-29 Amorphous alloys for electromagnetic devices
AT81107315T ATE21417T1 (de) 1980-09-26 1981-09-16 Amorphe legierungen fuer elektromagnetische geraete.
DE8181107315T DE3175108D1 (en) 1980-09-26 1981-09-16 Amorphous alloys for electromagnetic devices
EP81107315A EP0049770B1 (en) 1980-09-26 1981-09-16 Amorphous alloys for electromagnetic devices
AU75554/81A AU551753B2 (en) 1980-09-26 1981-09-22 Amorphous iron-based alloys for electromagnetic devices
KR1019810003573A KR890001340B1 (ko) 1980-09-26 1981-09-24 전자기 장치용 붕소함유 철기자성 합금
CA000386675A CA1181262A (en) 1980-09-26 1981-09-25 Amorphous alloys for electromagnetic devices
ES505808A ES8206642A1 (es) 1980-09-26 1981-09-26 Metodo de mejorar las propiedades magneticas de las aleacio-nes magneticas

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US19147580A 1980-09-26 1980-09-26
US06/286,918 US4409041A (en) 1980-09-26 1981-07-29 Amorphous alloys for electromagnetic devices

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EP (1) EP0049770B1 (es)
KR (1) KR890001340B1 (es)
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CA (1) CA1181262A (es)
DE (1) DE3175108D1 (es)
ES (1) ES8206642A1 (es)

Cited By (16)

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US4585480A (en) * 1984-04-03 1986-04-29 Hoganas Ab Material for the powder metallurgical manufacture of soft magnetic components
US4704169A (en) * 1982-09-08 1987-11-03 Hiroshi Kimura Rapidly quenched alloys containing second phase particles dispersed therein
US4834814A (en) * 1987-01-12 1989-05-30 Allied-Signal Inc. Metallic glasses having a combination of high permeability, low coercivity, low AC core loss, low exciting power and high thermal stability
US4889568A (en) * 1980-09-26 1989-12-26 Allied-Signal Inc. Amorphous alloys for electromagnetic devices cross reference to related applications
US5035755A (en) * 1984-05-23 1991-07-30 Allied-Signal Inc. Amorphous metal alloys having enhanced AC magnetic properties at elevated temperatures
US5278377A (en) * 1991-11-27 1994-01-11 Minnesota Mining And Manufacturing Company Electromagnetic radiation susceptor material employing ferromagnetic amorphous alloy particles
US5370749A (en) * 1981-02-17 1994-12-06 Allegheny Ludlum Corporation Amorphous metal alloy strip
US20030151487A1 (en) * 2002-02-08 2003-08-14 Ryusuke Hasegawa Filter circuit having an Fe-based core
US6749695B2 (en) 2002-02-08 2004-06-15 Ronald J. Martis Fe-based amorphous metal alloy having a linear BH loop
US6960860B1 (en) * 1998-06-18 2005-11-01 Metglas, Inc. Amorphous metal stator for a radial-flux electric motor
US20090030527A1 (en) * 2003-06-27 2009-01-29 Zuli Holdings, Ltd. Amorphous metal alloy medical devices
US20090189728A1 (en) * 2006-02-28 2009-07-30 Kazuyuki Fukui Amorphous transformer for electric power supply
US8382821B2 (en) 1998-12-03 2013-02-26 Medinol Ltd. Helical hybrid stent
US9039755B2 (en) 2003-06-27 2015-05-26 Medinol Ltd. Helical hybrid stent
US9155639B2 (en) 2009-04-22 2015-10-13 Medinol Ltd. Helical hybrid stent
US12478488B2 (en) 2020-02-19 2025-11-25 Medinol Ltd. Helical stent with enhanced crimping

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JPS6034620B2 (ja) * 1981-03-06 1985-08-09 新日本製鐵株式会社 鉄損が極めて低く熱的安定性とよい非晶質合金
DE3274562D1 (en) * 1981-08-21 1987-01-15 Allied Corp Metallic glasses having a combination of high permeability, low coercivity, low ac core loss, low exciting power and high thermal stability
US4473413A (en) * 1983-03-16 1984-09-25 Allied Corporation Amorphous alloys for electromagnetic devices
US4759949A (en) * 1987-07-23 1988-07-26 Westinghouse Electric Corp. Method of insulating ferromagnetic amorphous metal continuous strip
TW226034B (es) * 1991-03-06 1994-07-01 Allied Signal Inc
JP3302031B2 (ja) * 1991-09-06 2002-07-15 健 増本 高靭性高強度非晶質合金材料の製造方法
JP2954775B2 (ja) * 1992-02-14 1999-09-27 ワイケイケイ株式会社 微細結晶組織からなる高強度急冷凝固合金
JP2911673B2 (ja) * 1992-03-18 1999-06-23 健 増本 高強度アルミニウム合金
GB2319253A (en) * 1996-11-16 1998-05-20 Eric Leigh Mayes Composition, for use in a device, comprising a magnetic layer of domain-separated magnetic particles
US6815063B1 (en) 1996-11-16 2004-11-09 Nanomagnetics, Ltd. Magnetic fluid
US6986942B1 (en) 1996-11-16 2006-01-17 Nanomagnetics Limited Microwave absorbing structure
US6713173B2 (en) 1996-11-16 2004-03-30 Nanomagnetics Limited Magnetizable device
US20060180248A1 (en) 2005-02-17 2006-08-17 Metglas, Inc. Iron-based high saturation induction amorphous alloy
JP4843620B2 (ja) 2005-02-17 2011-12-21 メトグラス・インコーポレーテッド 鉄基高飽和磁気誘導アモルファス合金

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Cited By (32)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4889568A (en) * 1980-09-26 1989-12-26 Allied-Signal Inc. Amorphous alloys for electromagnetic devices cross reference to related applications
US5370749A (en) * 1981-02-17 1994-12-06 Allegheny Ludlum Corporation Amorphous metal alloy strip
US6471789B1 (en) 1981-02-17 2002-10-29 Ati Properties Amorphous metal alloy strip
US6277212B1 (en) 1981-02-17 2001-08-21 Ati Properties, Inc. Amorphous metal alloy strip and method of making such strip
US6296948B1 (en) 1981-02-17 2001-10-02 Ati Properties, Inc. Amorphous metal alloy strip and method of making such strip
US4704169A (en) * 1982-09-08 1987-11-03 Hiroshi Kimura Rapidly quenched alloys containing second phase particles dispersed therein
US4585480A (en) * 1984-04-03 1986-04-29 Hoganas Ab Material for the powder metallurgical manufacture of soft magnetic components
US5035755A (en) * 1984-05-23 1991-07-30 Allied-Signal Inc. Amorphous metal alloys having enhanced AC magnetic properties at elevated temperatures
US4834814A (en) * 1987-01-12 1989-05-30 Allied-Signal Inc. Metallic glasses having a combination of high permeability, low coercivity, low AC core loss, low exciting power and high thermal stability
US5278377A (en) * 1991-11-27 1994-01-11 Minnesota Mining And Manufacturing Company Electromagnetic radiation susceptor material employing ferromagnetic amorphous alloy particles
US6960860B1 (en) * 1998-06-18 2005-11-01 Metglas, Inc. Amorphous metal stator for a radial-flux electric motor
US8382821B2 (en) 1998-12-03 2013-02-26 Medinol Ltd. Helical hybrid stent
US20030151487A1 (en) * 2002-02-08 2003-08-14 Ryusuke Hasegawa Filter circuit having an Fe-based core
US6749695B2 (en) 2002-02-08 2004-06-15 Ronald J. Martis Fe-based amorphous metal alloy having a linear BH loop
US7541909B2 (en) 2002-02-08 2009-06-02 Metglas, Inc. Filter circuit having an Fe-based core
US9039755B2 (en) 2003-06-27 2015-05-26 Medinol Ltd. Helical hybrid stent
US20090030527A1 (en) * 2003-06-27 2009-01-29 Zuli Holdings, Ltd. Amorphous metal alloy medical devices
US10363152B2 (en) 2003-06-27 2019-07-30 Medinol Ltd. Helical hybrid stent
US7887584B2 (en) 2003-06-27 2011-02-15 Zuli Holdings, Ltd. Amorphous metal alloy medical devices
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AU7555481A (en) 1982-04-01
KR830007873A (ko) 1983-11-07
AU551753B2 (en) 1986-05-08
EP0049770A2 (en) 1982-04-21
EP0049770A3 (en) 1982-05-12
KR890001340B1 (ko) 1989-04-29
ES505808A0 (es) 1982-09-01
DE3175108D1 (en) 1986-09-18
ES8206642A1 (es) 1982-09-01
CA1181262A (en) 1985-01-22
EP0049770B1 (en) 1986-08-13

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